158 research outputs found
Anisotropy of the Stone-Wales Defect and Warping of Graphene Nano-ribbons: A First-principles Analysis
Stone-Wales (SW) defects, analogous to dislocations in crystals, play an
important role in mechanical behavior of -bonded carbon based materials.
Here, we show using first-principles calculations that a marked anisotropy in
the interaction among the SW defects has interesting consequences when such
defects are present near the edges of a graphene nano-ribbon: depending on
their orientation with respect to edge, they result in compressive or tensile
stress, and the former is responsible to depression or warping of the graphene
nano-ribbon. Such warping results in delocalization of electrons in the defect
states.Comment: 8 page
Sensory organ like response determines the magnetism of zigzag-edged honeycomb nanoribbons
We present an analytical theory for the magnetic phase diagram for zigzag
edge terminated honeycomb nanoribbons described by a Hubbard model with an
interaction parameter U . We show that the edge magnetic moment varies as ln U
and uncover its dependence on the width W of the ribbon. The physics of this
owes its origin to the sensory organ like response of the nanoribbons,
demonstrating that considerations beyond the usual Stoner-Landau theory are
necessary to understand the magnetism of these systems. A first order magnetic
transition from an anti-parallel orientation of the moments on opposite edges
to a parallel orientation occurs upon doping with holes or electrons. The
critical doping for this transition is shown to depend inversely on the width
of the ribbon. Using variational Monte-Carlo calculations, we show that
magnetism is robust to fluctuations. Additionally, we show that the magnetic
phase diagram is generic to zigzag edge terminated nanostructures such as
nanodots. Furthermore, we perform first principles modeling to show how such
magnetic transitions can be realized in substituted graphene nanoribbons.Comment: 5 pages, 5 figure
Interplay between Nitrogen Dopants and Native Point Defects in Graphene
To understand the interaction between nitrogen dopants and native point
defects in graphene, we have studied the energetic stability of N-doped
graphene with vacancies and Stone-Wales (SW) defect by performing the density
functional theory calculations. Our results show that N substitution
energetically prefers to occur at the carbon atoms near the defects, especially
for those sites with larger bond shortening, indicating that the defect-induced
strain plays an important role in the stability of N dopants in defective
graphene. In the presence of monovacancy, the most stable position for N dopant
is the pyridinelike configuration, while for other point defects studied (SW
defect and divacancies) N prefers a site in the pentagonal ring. The effect of
native point defects on N dopants is quite strong: While the N doping is
endothermic in defect-free graphene, it becomes exothermic for defective
graphene. Our results imply that the native point defect and N dopant attract
each other, i.e., cooperative effect, which means that substitutional N dopants
would increase the probability of point defect generation and vice versa. Our
findings are supported by recent experimental studies on the N doping of
graphene. Furthermore we point out possibilities of aggregation of multiple N
dopants near native point defects. Finally we make brief comments on the effect
of Fe adsorption on the stability of N dopant aggregation.Comment: 10 pages, 5 figures. Figure 4(g) and Figure 5 are corrected. One
additional table is added. This is the final version for publicatio
Synthesis, Structure and Properties of Boron and Nitrogen Doped Graphene
Two-dimensional graphene exhibits many fascinating properties such as
ballistic electronic conduction and quantum Hall effect at room temperature.1-4
Graphene doped electrochemically or through charge-transfer with electron-donor
and -acceptor molecules,5-7 shows marked changes in electronic structure, with
characteristic signatures in the Raman spectra.5-10 Substitutional doping,
universally used in tuning properties of semiconductors, could be a powerful
tool to control the electronic properties of graphene. Here, we present the
structure and properties of boron and nitrogen doped graphenes, obtained by
more than one method involving arc discharge in appropriate gaseous atmosphere,
by using modified graphite electrode or by the transformation of nano-diamond.
Using a combination of experiment and firstprinciples theory, we demonstrate
systematic changes in the carrier-concentration and electronic structure of
graphenes with B/N-doping, accompanied by stiffening of the Gband and
intensification of the defect related D-band in the Raman spectra. Such n/p -
type graphenes obtained without external fields or chemical agents should find
device applications.Comment: 12 pages, 5 figures, 1 tabl
Localized state and charge transfer in nitrogen-doped graphene
Nitrogen-doped epitaxial graphene grown on SiC(000?1) was prepared by
exposing the surface to an atomic nitrogen flux. Using Scanning Tunneling
Microscopy (STM) and Spectroscopy (STS), supported by Density Functional Theory
(DFT) calculations, the simple substitution of carbon by nitrogen atoms has
been identified as the most common doping configuration. High-resolution images
reveal a reduction of local charge density on top of the nitrogen atoms,
indicating a charge transfer to the neighboring carbon atoms. For the first
time, local STS spectra clearly evidenced the energy levels associated with the
chemical doping by nitrogen, localized in the conduction band. Various other
nitrogen-related defects have been observed. The bias dependence of their
topographic signatures demonstrates the presence of structural configurations
more complex than substitution as well as hole-doping.Comment: 5 pages, accepted in PR
Local density of states and scanning tunneling currents in graphene
We present exact analytical calculations of scanning tunneling currents in
locally disordered graphene using a multimode description of the microscope
tip. Analytical expressions for the local density of states (LDOS) are given
for energies beyond the Dirac cone approximation. We show that the LDOS at the
and sublattices of graphene are out of phase by implying that the
averaged LDOS, as one moves away from the impurity, shows no trace of the
(with the Fermi momentum) Friedel modulation. This means that a
STM experiment lacking atomic resolution at the sublattice level will not be
able of detecting the presence of the Friedel oscillations [this seems to be
the case in the experiments reported in Phys. Rev. Lett. {\bf 101}, 206802
(2008)]. The momentum maps of the LDOS for different types of impurities are
given. In the case of the vacancy, features are seen in these maps. In
all momentum space maps, and features are seen. The
features are different from what is seen around zero momentum. An
interpretation for these features is given. The calculations reported here are
valid for chemical substitution impurities, such as boron and nitrogen atoms,
as well as for vacancies. It is shown that the density of states close to the
impurity is very sensitive to type of disorder: diagonal, non-diagonal, or
vacancies. In the case of weakly coupled (to the carbon atoms) impurities, the
local density of states presents strong resonances at finite energies, which
leads to steps in the scanning tunneling currents and to suppression of the
Fano factor.Comment: 21 pages. Figures 6 and 7 are correctly displayed in this new versio
Chemical Modification of Graphene Oxide by Nitrogenation: An X-ray Absorption and EmissionSpectroscopy Study
Nitrogen-doped graphene oxides (GO:Nx) were synthesized by a partial reduction of graphene oxide (GO) using urea [CO(NH2)2]. Their electronic/bonding structures were investigated using X-ray absorption near-edge structure (XANES), valence-band photoemission spectroscopy (VB-PES), X-ray emission spectroscopy (XES) and resonant inelastic X-ray scattering (RIXS). During GO:Nx synthesis, different nitrogen-bonding species, such as pyrrolic/graphitic-nitrogen, were formed by replacing of oxygen-containing functional groups. At lower N-content (2.7 at%), pyrrolic-N, owing to surface and subsurface diffusion of C, N and NH is deduced from various X-ray spectroscopies. In contrast, at higher N-content (5.0 at%) graphitic nitrogen was formed in which each N-atom trigonally bonds to three distinct sp2-hybridized carbons with substitution of the N-atoms for C atoms in the graphite layer. Upon nitrogen substitution, the total density of state close to Fermi level is increased to raise the valence-band maximum, as revealed by VB-PES spectra, indicating an electron donation from nitrogen, molecular bonding C/N/O coordination or/and lattice structure reorganization in GO:Nx. The well-ordered chemical environments induced by nitrogen dopant are revealed by XANES and RIXS measurements
A hybrid MBE-based growth method for large-area synthesis of stacked hexagonal boron nitride/graphene heterostructures
Van der Waals heterostructures combining hexagonal boron nitride (h-BN) and graphene offer many potential advantages, but remain difficult to produce as continuous films over large areas. In particular, the growth of h-BN on graphene has proven to be challenging due to the inertness of the graphene surface. Here we exploit a scalable molecular beam epitaxy based method to allow both the h-BN and graphene to form in a stacked heterostructure in the favorable growth environment provided by a Ni(111) substrate. This involves first saturating a Ni film on MgO(111) with C, growing h-BN on the exposed metal surface, and precipitating the C back to the h-BN/Ni interface to form graphene. The resulting laterally continuous heterostructure is composed of a top layer of few-layer thick h-BN on an intermediate few-layer thick graphene, lying on top of Ni/MgO(111). Examinations by synchrotron-based grazing incidence diffraction, X-ray photoemission spectroscopy, and UV-Raman spectroscopy reveal that while the h-BN is relaxed, the lattice constant of graphene is significantly reduced, likely due to nitrogen doping. These results illustrate a different pathway for the production of h-BN/graphene heterostructures, and open a new perspective for the large-area preparation of heterosystems combining graphene and other 2D or 3D materials
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